Comprehensively enhanced energy-storage properties in (Pb1−3x/2Lax)(Zr0.995Ti0.005)O3 antiferroelectric ceramics via composition optimization

Abstract

Antiferroelectric materials as one of the front candidates for high energy storage capacitors should in principle combine a small hysteresis width, high breakdown strength, large phase switching and high polarization. However, the simultaneous optimization of these parameters is a long-standing challenge. Herein, we present a superior energy storage performance of (Pb_1−3x/2La_x)(Zr_0.995Ti_0.005)O₃ antiferroelectric ceramics by composition optimization. Although La³⁺ doping reduces the maximum polarization, the refined grain size and increased band gap ensure high breakdown strength, and the enhanced antiferroelectric state and induced relaxation behavior lead to high phase-switching fields and a small hysteresis width, respectively. As a result, an optimal recoverable energy density of 12.3 J cm⁻³ and a high efficiency of 84% are achieved simultaneously under 42 kV mm⁻¹ in the (Pb_0.925La_0.05)(Zr_0.995Ti_0.005)O₃ ceramic, resulting in a remarkable energy storage performance that exceeds most antiferroelectric ceramics. Additionally, this ceramic also has a pretty excellent energy density (>8 J cm⁻³) under temperatures from 60 to 120 °C and frequencies from 1 to 100 Hz. All features highlight (Pb_0.925La_0.05)(Zr_0.995Ti_0.005)O₃ ceramics as a potential candidate for high energy storage applications.